Abstract
While carbene complexes of uranium have been known for over a decade, there are no reported examples of complexes between an actinide and a "heavy carbene." Here we report the syntheses and structures of the first uranium-heavy tetrylene complexes: (CpSiMe3)3U-Si[PhC(NR)2]R' (R = t Bu, R' = NMe21; R = i Pr, R' = PhC(N i Pr)22). Complex 1 features a kinetically robust uranium-silicon bonding interaction, while the uranium-silicon bond in 2 is easily disrupted thermally or by competing ligands in solution. Calculations reveal polarized σ bonds, but depending on the substituents at silicon a substantial π bonding interaction is also present. The complexes possess relatively high bond orders which suggests primarily covalent bonding between uranium and silicon. These results comprise a new frontier in actinide-heavy main group bonding.
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